Miscible polyolefin blends

The invention relates to melt-miscible polyolefin blends, and a process for preparing the melt-miscible blends, of two or more polyolefins. Matching, within defined limits, the segment length of a modifying polyolefin with the segment length of a primary polyolefin, such as polypropylene or an ethylene/alpha-olefin copolymer, provides blends of the "matched" components which blends were heretofore unknown to be melt-miscible. A broad range of polyolefin blend compositions, and of polyolefin blends containing other polymers made compatible or dispersible with the polyolefin blend compositions, are defined, all of the blend compositions having at least one melt-miscible polyolefin phase.

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Claims

1. A polyolefin blend, comprising:

a) a primary polyolefin having a primary polyolefin segment length, wherein said primary polyolefin is polypropylene; and
b) at least one modifying polyolefin comprising a random copolymer of ethylene and one or more monomer units selected from the group consisting of a lower olefin, a lower diolefin, and mixtures thereof, wherein the modifying polyolefin has a modifying polyolefin segment length within 90% to 110% of the primary polyolefin length.

2. The polyolefin blend of claim 1 wherein:

a) the segment length of the primary polyolefin is within a range of absolute value of from about 4.2 to about 8.8 Angstroms;
b) the modifying polyolefin comprises ethylene and one or more monomer units selected from the group consisting of propylene, 1-butene, butadiene, 1-pentene, 1-hexene, 1-octene, isoprene, 2-methyl-1-butene, 3-methyl-1-butene, 4-methyl-1-pentene, and mixtures thereof;
and further wherein the range and the absolute value of the primary olefin segment length and the modifying polyolefin segment length are determined from an arbitrarily chosen common segment volume of 1.08.times.10.sup.-22 cubic centimeters.

3. The polyolefin blend of claim 1 wherein the primary polyolefin segment length ("SL-1") and the modifying polyolefin segment length ("SL-X") have a relationship:

4. The polyolefin blend of claim 1 wherein the primary polyolefin has a weight average molecular weight (Mw) up to about 300,000 daltons and the modifying polyolefin has a Mw up to about 1,000,000 daltons.

5. The polyolefin blend of claim 1 wherein the primary polyolefin has a weight average molecular weight (Mw) up to about 600,000 daltons and the modifying polyolefin has a Mw up to about 750,000 daltons.

6. The polyolefin blend of claim 2 wherein the modifying polyolefin is a copolymer of ethylene and one or more monomer units selected from the group consisting of propylene, 1-butene, butadiene, isoprene, 2-methyl-1-butene, and 3-methyl-1-butene.

7. The polyolefin blend of claim 2 wherein the modifying polyolefin has at least one terminal functional fragment derived from a reactive terminal molecule selected from the group consisting of carbon dioxide, ethylene oxide, propylene oxide, succinic anhydride, maleic anhydride, glutaric anhydride, epichlorohydrin, caprolactone, and halide.

8. The polyolefin blend of claim 6 wherein the modifying polyolefin is a copolymer of ethylene, and 1-butene, butadiene, or isoprene.

9. The polyolefin blend of claim 8 wherein the weight average molecular weight (Mw) of the polypropylene is up to about 300,000 daltons, and the modifying polyolefin is a poly(ethylene/1-butene) copolymer comprising from about 12 to about 41 weight % ethylene and from about 59 to about 88 weight % 1-butene, and having a Mw of up to about 730,000 daltons.

10. The polyolefin blend of claim 9 wherein the poly(ethylene/1-butene) is a copolymer of about 18 to about 34 weight % ethylene and from about 66 to about 82 weight % 1-butene and is prepared by hydrogenating anionically polymerized butadiene.

11. The polyolefin blend of claim 6 wherein the weight average molecular weight (Mw) of the polypropylene is up to about 300,000 daltons and the modifying polyolefin has a segment length within about 90 to about 110% of the polypropylene segment length and comprises a poly{ethylene-propylene (EP)/isopropylethylene (iPE)/methylethylethylene (MEE)} random copolymer comprising from about 0 to about 81 weight % ethylene-propylene, from about 16 to about 62 weight % isopropylethylene, and from about 0 to about 84 weight % methylethylethylene, and has a Mw of up to about 66,000 daltons.

12. The polyolefin blend of claim 6 wherein the weight average molecular weight (Mw) of the polypropylene is up to about 300,000 daltons and the modifying polyolefin has a Mw of up to about 430,000 daltons, a segment length within about 95 to about 105% of the polypropylene segment length, and comprises a poly{ethylene-propylene (EP)/isopropylethylene (iPE)/methylethyl-ethylene (MEE)} random copolymer prepared by hydrogenating anionically polymerized isoprene.

13. A polyolefin blend having at least one melt-miscible polyolefin blend phase, the polyolefin blend comprising:

a) a primary polyolefin selected from the group consisting of polypropylene and an ethylene/alpha-olefin copolymer having a defined segment length (SL-1) within a range of absolute value of from about 4.2 to about 8.8 Angstroms; and
b) at least one modifying polyolefin comprising a block copolymer having two blocks, each block being a polymer of ethylene and one or more monomer units selected from the group consisting of propylene, 1-butene, butadiene, 1-pentene, 1-hexene, 1-octene, isoprene, 2-methyl-1-butene, 3-methyl-1-butene, 4-methyl-1-pentene, and mixtures thereof,
wherein each block of the modifying polyolefin has a weight average molecular weight of at least 20,000 daltons,
and wherein the melt-miscible polyolefin blend phase comprises at least one block having a block segment length (SL-B) of from about 85% to about 115% of the SL-1,
and further wherein the SL-1 range and the absolute value of SL-1 and SL-B are determined from an arbitrarily chosen common segment volume of 1.08.times.10.sup.-22 cubic centimeters.

14. The polyolefin blend of claim 13 wherein at least one of the two blocks comprises a terminal functional fragment derived from a reactive terminal molecule selected from the group consisting of carbon dioxide, ethylene oxide, propylene oxide, succinic anhydride, maleic anhydride, glutaric anhydride, epichlorohydrin, caprolactone, and allyl halide.

15. A polyolefin blend having a melt-miscible polyolefin blend phase, the polyolefin blend comprising:

a) a primary polyolefin selected from the group consisting of polypropylene and an ethylene/alpha-olefin copolymer having a segment length (SL-1) within a range of absolute value of from about 4.2 to about 8.8 Angstroms; and
b) at least one modifying polyolefin comprising a block/segment copolymer comprising:
i. a block being a polymer of ethylene and one or more monomer units selected from the group consisting of propylene, 1-butene, butadiene, 1-pentene, 1-hexene, 1-octene, isoprene, 2-methyl-1-butene, 3-methyl-1-butene, 4-methyl-1-pentene, and mixtures thereof, and
ii. at least one segment comprising a polar polymer having a weight average molecular weight of at least 1,000 daltons, the polar polymer segment derived from monomer units selected from the group consisting of styrene, substituted styrene, vinyl pyridine, N-vinyl pyrrolidone, a C.sub.1 -C.sub.8 alkyl acrylic ester, a C.sub.1 -C.sub.18 methacrylic ester, phenyl methacrylate, benzyl methacrylate, acrylonitrile, methacrylonitrile, and mixtures thereof;
wherein the block has a segment length (SL-B) of from about 85% to about 115% of the SL-1, and wherein an absolute value of the SL-1 and the SL-B is determined from a chosen common segment volume of 1.08.times.10.sup.-22 cubic centimeters, and further wherein the block/segment copolymer has a weight average molecular weight of at least 20,000 daltons.

16. The polyolefin blend having a melt-miscible polyolefin blend phase according to claim 15 wherein the block further comprises a terminal functional fragment derived from a reactive terminal molecule selected from the group consisting of carbon dioxide, ethylene oxide, propylene oxide, succinic anhydride, maleic anhydride, glutaric anhydride, epichlorohydrin, caprolactone, and allyl halide.

17. The polyolefin blend having a melt-miscible polyolefin blend phase according to claim 15 wherein the derived polar polymer segment of the modifying polyolefin further comprises a reactive monomer unit selected from the group consisting of acrylic acid, methacrylic acid, crotonic acid, itaconic acid, maleic acid, maleic anhydride, fumaric acid, hydroxyethyl methacrylate, hydroxypropyl methacrylate, tertiarybutylaminoethyl methacrylate, dimethylaminoethyl methacrylate, glycidyl methacrylate, methacryloxypropyl triethoxysilane, acryloxyproprionic acid, caprolactone, and mixtures thereof.

18. The polyolefin blend having a melt-miscible polyolefin blend phase according to claim 17 wherein the block of the modifying polyolefin further comprises a terminal functional fragment derived from a reactive terminal molecule selected from the group consisting of carbon dioxide, ethylene oxide, propylene oxide, succinic anhydride, maleic anhydride, glutaric anhydride, epichlorohydrin, caprolactone, and allyl halide.

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Patent History
Patent number: 5710219
Type: Grant
Filed: Sep 23, 1994
Date of Patent: Jan 20, 1998
Assignee: Regents of the University of Minnesota (Minneapolis, MN)
Inventors: Frank S. Bates (St. Louis Park, MN), Jeffrey H. Rosedale (Philadelphia, PA), Mark F. Schulz (Minneapolis, MN), Kristoffer Almdal (Roskilde)
Primary Examiner: Helen Lee
Law Firm: Mueting, Raasch, Gebhardt & Schwappach, P.A.
Application Number: 8/311,410